2 Answers
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Amarok is set up to use the X keycode "Media play" as a global shortcut for play/pause. Sometimes, however, your keyboard configuration may not be properly recognized for whatever reason - in which case, you can specify it manually. To do this, follow the instructions below:

Open Amarok

Select "Settings" from the menu and choose the "Configure shortcuts" submenu.

Type "play" in the filter box, this will filter display all possible shortcuts that has the word "play" in it.

You will see a few items named something with "play", and one of them will be "Play/pause".

You will also see three columns: "Shortcut", "Alternate" and "Global". The two first are valid only when Amarok is in focus - that means whenever you are inside Amarok and fiddling around. The "Global" keyboard shortcut, however, will work regardless of whether Amarok is minimized, in the notification area or you have it open.

Press the little triangle in the "Global" column for the "play/pause" entry. This may already have the words "Media play" shown (this is the current shortcut for this action - if you have a proper media keyboard, the "play" button will usually trigger this action in Amarok).

With the entry now expanded, click the button after "Custom" that says "None". When you have clicked it, it is in "recording" mode, so press the key you want to be assigned to this function. When it is released, it should show up on the button you just clicked, next to the text "Custom". Make sure this also selects the radio box for "Custom" and then click "Apply".